Composite powder and cosmetic containing the same

ABSTRACT

A first subject of the present invention is a composite powder having antibacterial and antifungal effect, in which a base powder, zinc oxide and/or zinc basic carbonate, and alkali metal salt are combined. 
     In the composite powder, it is preferable that the base powder is an adsorbing site for adsorbing a specified enzyme, and a site in which zinc oxide and/or zinc basic carbonate and alkali metal salt are combined is an acting site having enzyme inhibiting or activating property. 
     In the composite powder, it is preferable that the zeta-potential of an adsorbing site at pH to be used is a negative value, and the zeta-potential of an adsorbing site at pH 7.5 is −10 mV or lower. 
     A second subject of the present invention is a cosmetic composition comprising the aforementioned composite powder. 
     The composite powder can be also used as a skin roughening improving agent, a sensitive skin caring agent or a pimpled skin caring agent.

RELATED APPLICATIONS

This application claims priority to the Japanese Patent ApplicationNos.2002-96254 filed on Mar. 29, 2002 and 2002-96255 filed on Mar. 29,2002 and 2002-355790 filed on Dec. 6, 2002 and 2002-355789 filed on Dec.6, 2002 is hereby incorporated with reference for all purposes.

BACKGROUND OF THE INVENTION

1. Field of the Invention

This invention relates to composite powder and cosmetic compositioncontaining the same, in particular, their improvement of theantibacterial and antifungal activity, and also relates to a compositepowder having both of plasminogen activator (PA) inhibitory activity andantibacterial and antifungal activity and a cosmetic containing thesame.

2. Prior Art

Many kinds of antibacterial and antifungal agents are used in extremelywide area in the human life (food, clothing and shelter). These agentsare typically divided into organic group and inorganic group.

Organic antibacterial and antifungal agents include paraben, triclosan,quaternary ammonium salt, chlorhexidine hydrochloride, thiabendazole,carbenedazine, captan, fluorofolpet, chlorothalonil and so on.

On the other hand, inorganic antibacterial and antifungal agents mainlyinclude silicate, phosphate, zeolite, synthetic mineral and so on,retaining or substituting with antibacterial metals such as inparticular silver, copper, and zinc. Among them, for example, silver- orzinc-substituted zeolite, silver-retaining apatite, silver-retainingsilica gel and so on are put to practical use.

These antibacterial and antifungal agents could prevent products frombacterial or fungal infection, contamination, and deterioration by usingthem in the preparation of construction materials, daily necessities andso on. However, it rarely happened that these antibacterial andantifungal agents possess stimulation on human bodies.

On the other hand, not only morbid dermatitis such as atopic dermatitisand severe pimpled skin, but also so-called sensitive skin exhibitinghypersensitive response to environmental change although it is notmorbid, are problematic and, when an antibacterial and antifungal agentis used in a composition which is directly applied to a human body suchas cosmetic compositions, safe and mildly stimulative antibacterial andantifungal agent is demanded.

Since the organic antibacterial and antifungal agents such as parabenand the like which are commonly used as preservatives of cosmeticcompositions have possibility to show skin stimulative action, it havebeen desired to develop excellent inorganic antibacterial and antifungalagents.

Conventional inorganic antibacterial and antifungal agents, comparedwith organic ones, are safe for human body and are hard to be influencedby heat, chemical agents, and so on. However these inorganic agentsgenerally show rather low antifungal activity. Accordingly thedevelopment of inorganic agents possessing excellent antibacterial andantifungal activities has been desired.

SUMMARY OF THE INVENTION

The present invention was done in view of the aforementioned previousproblems, and an object thereof is to provide a composite powder havingexcellent antibacterial and antifungal activity besides plasminogenactivator inhibitory activity, and a cosmetic containing the same.

In view of the aforementioned problems, the present inventorsintensively studied and found out that a composite powder containingzinc oxide and/or zinc basic carbonate and alkali metal salt hasexcellent antiseptic effect even when an small amount of an organiccomposite powder such as paraben or none of the powder is used. Further,the present inventors found out that excellent PA inhibiting effect isexerted, in addition to antibacterial and antifungal activity bycombining an acting site comprising zinc oxide and/or zinc basiccarbonate and alkali metal salt with an adsorbing site which adsorbs aspecified enzyme.

That is, a first subject of the present invention is a composite powderhaving antibacterial and antifungal effect, in which a base powder, zincoxide and/or zinc basic carbonate, and alkali metal salt are combined.

In the composite powder, it is preferable that the base powder is anadsorbing site for adsorbing a specified enzyme, and a site, in whichzinc oxide and/or zinc basic carbonate and alkali metal salt arecombined, is an acting site having enzyme inhibiting or activatingproperty.

It is preferable that the composite powder is in a form in which surfaceof the base powder is covered with zinc oxide and/or zinc basiccarbonate and alkali metal salt in stripe or spot state;

-   -   in a form in which a surface of the base powder is covered with        zinc oxide and/or zinc basic carbonate and alkali metal salt in        net state;    -   in a form in which zinc oxide and/or zinc basic carbonate and        alkali metal salt are encapsulated, embedded or included in the        base powder.

In addition, in the composite powder, it is preferable that an actingsite and an adsorbing site are formed on an inactive powder in stripe orspot state.

In the composite powder, it is preferable that alkali metal salt isencapsulated, embedded or included in zinc oxide and/or zinc basiccarbonate.

In the composite powder, it is preferable that the specified enzyme isplasminogen activator, and the acting site is a site having plasminogenactivator inhibitory property.

In the composite powder, it is preferable that the alkali metal salt is1 or more than 2 selected from the group consisting of hydroxide,hydrogen carbonate and carbonate of lithium, sodium and potassium.

In the composite powder, it is preferable that the zeta-potential of anadsorbing site is a negative value at used pH, and the zeta-potential ofan adsorbing site at pH 7.5 is −10 mV or lower.

In the composite powder, it is preferable that the adsorbing site is 1or more than 2 selected from the group consisting of silica, talc, mica,polyamide, polymethyl methacrylate or silicone resin.

In the composite powder, it is preferable that a content of alkali metalsalt is 0.5 to 50% by weight relative to the whole powder, and a contentof zinc oxide and/or zinc basic carbonate is 5 to 75% by weight relativeto the whole powder.

In the composite powder, it is preferable that, as a raw material forsynthesizing zinc oxide and/or zinc basic carbonate, zinc acetate, zincchloride or zinc sulfate containing acetic acid at the same time isused.

In the composite powder, it is preferable that an inhibiting rate ofplasminogen activator is 40% or larger.

An inhibiting rate of plasminogen activator (PA) is measured by thefollowing method: An inhibiting rate of urokinase (UK) that is a kind ofPA is measured.

Assessment is performed by measurement of activity of a buffercontaining 0.1% of a test sample and double-stranded UK-type PA (30U/mL). The activity means degradation activity of both samples tosynthetic substrate.

It is preferable that pH of 10% by weight of the composite powderdispersion in water is 9 to 14.

It is preferable that the composite powder is obtained by continuouslysupplying an aqueous solution containing zinc ion and an alkali aqueoussolution to a reactor containing a base powder while amounts of the twoaqueous solutions to be added dropwise are adjusted so that pH of thereaction solution is retained constant between 7 to 10 under roomtemperature and atmospheric pressure, and filtering the product,followed by washing with water and drying.

A second subject of the present invention is a cosmetic compositioncomprising the aforementioned composite powder.

It is preferable that the cosmetic composition does not substantiallycontain other antibacterial and antifungal agent.

The composite powder can be also used as a skin roughening improvingagent, a sensitive skin caring agent or a pimpled skin caring agent.

BRIEF DESCRIPTION OF THE DRAWINGS

FIG. 1 is a view showing an example of the structure of the compositepowder according to this invention.

FIG. 2 is a view showing a different example of the structure of thecomposite powder according to this invention.

FIG. 3 is a view showing a different example of the structure of thecomposite powder according to this invention.

FIG. 4 is a view showing an example of the process of making thecomposite powder according to this invention.

FIG. 5 is a view showing the evaluation method of the antibacterialactivity of the composite powder according to this invention.

FIG. 6 is a view showing a relationship between pH of an aqueousdispersion of the composite powder of the present invention andmoldproofing activity against blue mold.

DESCRIPTION OF THE PREFERRED EMBODIMENT

Preferable embodiments of the present invention will be explained below.

The composite powder of the present invention is such that a basepowder, zinc oxide and/or zinc basic carbonate, and alkali metal saltare combined.

As the combined state, the state where a surface of a base powder iscovered in stripe or spot state with zinc oxide and/or zinc basiccarbonate, and alkali metal salt;

-   -   the state where a surface of a base powder is covered in net        state with zinc oxide and/or zinc basic carbonate, and alkali        metal salt 14;    -   and the state where zinc oxide and/or zinc basic carbonate, and        alkali metal salt are encapsulated, embedded or included in a        base powder ; are preferable. However, the state is not limited        to them as far as the effect of the present invention is not        deteriorated. Further, it is preferable that alkali metal salt        is encapsulated, embedded or included in zinc oxide and/or zinc        basic carbonate.        Zinc Oxide and/or Zinc Basic Carbonate

A synthesizing method of zinc oxide and/or zinc basic carbonate in thecomposite powder of the present invention is roughly classified into awet method in which synthesis is performed in an aqueous solution, and adry method in which a solution does not directly intervene. In the wetmethod, zinc basic carbonate can be generally obtained by mixing anaqueous solution containing a zinc ion and an alkali aqueous solutioncontaining a carbonate ion, and washing the product with water, followedby filtration and drying. This can be further fired to obtain zincoxide.

In addition, in the wet method, when a strong alkali aqueous solutionsuch as sodium hydroxide and potassium hydroxide is used in place of analkali aqueous solution containing a carbonate ion, this can be washedwith water, and filtered and dried to obtain zinc oxide, since zincoxide is directly synthesized not via zinc basic carbonate.

On the other hand, as the dry method, there are methods of heating metalzinc in the air (French method) and methods of heating Franklinite witha reducing agent such as a coal and a coke (American method), or thelike.

Alkali Metal Salt

The composite powder of the present invention contains alkali metalsalt. Specifically, it is preferable that the composite powder contains1 or more than 2 alkali metal salt(s) selected from hydroxide, hydrogencarbonate and carbonate of lithium, sodium and potassium. In addition,it is preferable that the alkali metal salt is sodium carbonate orpotassium carbonate. The composite powder can contain 1 or more than 2of the aforementioned alkali metal salt(s).

Base Powder

Since the zinc oxide and/or zinc basic carbonate is a fine particle, itbecomes difficult to spread in the case of blending it in a cosmetic ata large amount. However, by combining with a base powder having betterusability, this defect can be overcome.

As a base powder the following thing can be listed.

Inorganic Base Powder

As an inorganic base powder, kaolin group such as kaolinite, dickite,nacrite, haloidsite, antigorite, chrysotile and so on; smectite groupsuch as pyrophyllite, montmorillonite, nontronite, saponite, hectorite,bentonite and so on; illite group such as sericite, muscovite, lithiamica, synthetic mica and so on; silicate such as beidellite, aluminumsilicate magnesium and so on; calcium compound such as phosphoric acid 3calcium, hydroxyapatite and so on; magnesium silicate group such astalc, serpentine and so on; single component powder such as silica,alumina and so on; hard capsule such as zeolite, silicone powders, glasspowders, glass beads, titanium oxide-involving-silica, zincoxide-involving-silica, iron oxide-involving-silica, ceriumoxide-involving-silica, titanium oxide-involving-PMMA(polymethylmethacrylate), zinc oxide-involving-PMMA, cerium oxide-involving-PMMAand so on; pearl pigment such as titanated mica, titanium oxide-bariumsulfate, titanium oxide-tantalum, bismuth oxychloride, bismuthoxychloride-mica and so on can be listed.

Organic Base Powder

As an organic base powder, nylon powder, polyethylene powders, Teflon™powders, polypropylene powders, silk powders, vinyl acetate powders,methacrylate powders, poly acrylonitrile powders, polystyrene powders,cellulose powder, and so on are listed.

Inorganic Pigment Base Powder

As an inorganic pigment base powder, white pigment such as titaniumoxide, zinc oxide, zirconium oxide, cerium oxide and these complexoxides, and iron oxide, hydration iron oxide, chromium oxide, chromiumhydroxide, ultramarineblue, deep blue, oxidation cobalt and so on arelisted.

Organic Pigment Base Powder

As an organic pigment base powder, organic pigment such as Lithol RubineB, Lithol Rubine***, Lake Red CBA, Lithol Red, Deep Maroon, HelindonePink CN, Permaton Red, Permanent Red F5R, Permanent Orange, Benzidineorange G, Orange II, Hanza Yellow and Phthalocyanine Blue; zirconium,barium or aluminum lake such as Erythrosine, Phloxine B, Acid Red, FastAcid Magenta, Eosine YS, Eosine YSK, Violamine R, Oil Red XO, Orange II,Tartrazine, Sunset Yellow FCF, Uranine, Uranin K, Quinaline Yellow WS,Fast Green FCF and Brilliant Blue FCF and so on are listed.

In the composite powder of the present invention, when the base powderacts as an adsorbing site to adsorb a specified enzyme, when a siteactive at which zinc oxide and/or zinc basic carbonate and alkali metalsalt are combined, is an active site having the property of inhibitingor activating the enzyme, excellent PA inhibiting effect in addition toantibacterial and antifungal activity is exerted.

It is considered that a protein degrading enzyme (protease) in theepidermis cell plays an important role in normal process of keratinizinga skin, and it has been revealed that particularly change of activity offibrinogenolysis proteases such as plasmin and plasminogen activator hasparticularly deep relation to the formation of disease images of variousskin diseases. Plasmin is a protease whose precursor plasminogen hasbeen activated by PA, and plays an important role in inhibition ofthrombus formation in blood coagulation system, but it is known thatwhen plasmin is overproduced, a harmful peptide which destructs a tissueor a cell by its non-specific protein degrading action, or can be acause for inflammation or anaphylaxis shock such as dilation of bloodcapillary, sthenia of blood vessel permeability, constriction of smoothmuscle, and pain is produced, influencing adversely on a living body. Inaddition, it has been reported that urokinase (UK) which is one of PAhas activity of exasperating cell proliferation.

Examples of skin disease in which change in activity of fibrinolysisprotease is confirmed including psoriasis and pemphigus vulgaris whichis representative of inflammatory abnormal keratosic disease. Inpsoriasis, strong PA activity is confirmed at a parakeratosis site ofthe affected epidermis (Hibino et el.: Blood and Vessel; 17(6), 1986)and, in pemphigus vulgaris, PA produced in large amount in epidermiscell converts extracellular plasminogen into plasmin, and this plasmindigests a substance binding cells, whereby, a tissue fluid is pooledamong cells, and intraepidermal bulla is formed (Morioka S.: J.Invest.Dermatol;76, 1981). In addition, it has been reported that in a skin inwhich epidermal cell is abnormally proliferated by stimulation such ascleanser, etc., and skin roughening is caused, plasminogen which shouldbe originally localized around epidermal basal layer is activated by PA,and is dispersed as active plasmin in whole epidermal layer (Kitamura etal: Journal of Cosmetic Technology;29(2), 1995). From the foregoing, ithas been thought that, in order to improve or prevent various skindiseases or proliferating abnormality of an epidermal cell, it isimportant to control activity of PA. However, in the formerantibacterial and antifungal agents, no agent having skin diseaseimproving or preventing effect has been reported.

Structure of Composite Powder

In the composite powder 10 of the present invention, as typically shownin FIG. 1A, adsorbing site 12 is covered in stripe state or in spotstate with an acting site 14.

In addition, as shown in FIG. 1B, the acting site 14 is covered instripe state or in spot state with an adsorbing site 12. Alternatively,as shown in FIG. 1C, the adsorbing site 12 is formed on whole surface ofan acting site 14 in net state.

Further, examples of the composite powder 10 of the present inventioninclude various types of composite powder which are: composite powder 10in which an acting site 14 and an adsorbing site 12 are formed on a basepowder 16 (FIG. 2A); the composite powder in which an acting site14 iscarried between layers of adsorbing site 12 (FIG. 2B) (or compositepowder in which adsorbing site 12 is carried between layers of actingsite 14 (FIG. 2C)), and the composite powder 10 in which acting site 14is encapsulated in an adsorbing site 12 (FIG. 3A) (or composite powderin which an adsorbing site 12 is encapsulated in acting site 14 (FIG.3B). However, as far as the effect of the present invention is notdeteriorated, the structure of composite powder10 is not particularlylimited.

In the composite powder, it is preferable that the covering amount andthe covering rate are adjusted, so that such structure is obtained thatacting effect at the acting site can be sufficiently exerted, andadsorbing effect at the adsorbing site is not prevented.

Adsorbing Site

In the composite powder of the present invention, an adsorbing site isdetermined by a relationship with an enzyme to be adsorbed, and ispreferably assessed by correlation with the zeta-potential of a subjectenzyme.

When a powder has a charge in a liquid, an ion with the opposite chargeis attracted to the powder by an electrostatic force in order to cancelthis charge, and to form an electric double layer. A potential on anoutermost side of a double layer is a zeta-potential. Therefore, thezeta-potential is suitably used for assessing surface charge state of asubject, and ability to electrically adsorb an enzyme can be assessed.

The zeta-potential is obtained by Smoluchowski's equation:Zeta-potential=4πηU/ε

(η:viscosity of solvent, U:electrophoresis mobility, ε:inductivity ofsolvent).

In order to obtain the zeta-potential, a speed (V) and anelectrophoresis mobility (U) of a colloid particle are obtained by anelectrophoresis method. When electric field (E) is applied to a chargedcolloid particle, a particle is moved. V and U are obtained by V=L/t (L:moved distance, t: time) and U=V/E.

When a subject enzyme is plasminogen activator with a positive value ofthe zeta-potential, it is preferable that the zeta-potential of asubstance constituting an adsorbing site exhibits a negative value at pHon a skin. In addition, the zeta-potential value of a substanceconstituting an absorbing site exhibits preferably −10 mV or lower, morepreferably −15 mV or lower, most preferably −20 mV or lower at pH 7.5.

A method of measuring the zeta-potential is as follows:

A sample was dispersed in a Tris-HCl buffer of pH7.5, and subjected toultrasonic treatment, which was used for measurement. The zeta-potentialis measured using an electrophoresis light scattering photometerLEZA-600 manufactured by Otsuka Electronics Co., Ltd. Measurement isperformed three times, and the result is expressed as an average valuethereof.

A relationship between the zeta-potential of a main substance at pH 7.5,and UK (urokinase which is one of PA) adsorption rate at theconcentration of 100 ppm is shown below.

Zeta UK potential adsorption Sample (mV) rate (%) Inorganic powderSilica (SUNSPHERE L ™) −20.0 82 Mica (EIGHT PEARL 300S ™) −18.9 79 Talc(Talk JA-68R ™) −19.3 78 Zinc oxide (ZINC WHITE SEIDO) +5.5 29 Alumina(MAX LIGHT A100 ™) +17.3 0 Organic powder Polyamide (NYLON SP500 ™)−32.0 34 Polymethyl methacrylate (GANZPEARL ™) −18.0 42 Silicone resin(TOSPEARL 145A ™) −14.0 30 Ethyl carbamate (PLASTIC POWDER ™) −13.0 27Organo polysiloxane extremer spherical −12.0 18 powder (TREFIL E506S ™)Cellulose (CELLUFLOW C-25 ™) −2.0 21 Polyethylene (FLO-THENE UF ™) +1.010

A method of measuring UK adsorption rate is as follows:

A Tris-HCl buffer (pH7.5) was added to 20 μL of a suspension of a samplein water to a total amount of 180 μL, and 20 μL of 10 μg/mLprecursor-type UK was added thereto, and allowed to stand at roomtemperature for 5 minutes. Thereafter, the sample powder was filtered,and the filtrate was recovered. Further, the powder was sufficientlywashed with a constant amount of Tris-HCl buffer, and the filtrate andthe washing solution were combined, which was used as an unadsorbed UKsolution. The UK concentration in the unadsorbed UK solution is obtainedby ELISA method using TintEliza uPA (biopool), an amount of UK adsorbedonto a sample powder was calculated and a UK adsorption rate isobtained.

There is a tendency that as the zeta-potential is lower, a UK adsorptionrate is higher, and it was shown that there is a relationship betweenthe zeta-potential and a UK adsorption rate although among each organicpowder or each inorganic powder there is not necessarily proportionalrelationship.

Therefore, as preferable substances for an adsorbing site, inorganicpowders such as silica, mica, talc and so on; organic powders such aspolyamide, polymethyl methacrylate, silicone resin and so on arespecifically listed.

An adsorbing site may be composed of 1 or more than 2 substances.

Acting Site

In the composite powder of the present invention, an acting site is alsodetermined by a relationship with an enzyme of an action subject.

In the case where the subject enzyme is plasminogen activator, it ispreferable that, as a main component of an acting site, a metal or ametal compound from which a zinc ion is dissolved out is used.

Examples of a metal compound from which zinc ion is dissolved outinclude inorganic compounds in a form (complex) including oxide,hydroxide, nitrate, chloride, hydrate, carbonate, bicarbonate, sulfate,borate, persulfate and an inorganic compound (complex) containing themin the molecule; organic acid salts such as glycerophosphate, acetate,hydroxide and α-hydroxy acid (citrate, tartrate, lactate, malate) orfruit acid salt, amino acid salt (asparate, alginate, glycolate,fumarate) or fatty acid salt (palmitate, oleate, caseinate, behenate).When the composite powder of the present invention is used in a skinexternal preparation, examples of a particularly preferable metalcompound include zinc oxide and/or zinc basic carbonate.

Then, UK inhibiting rates of ions at the ion concentration of 100 ppmare shown.

Sample UK active inhibition rate (%) Zn2+ 52 Zr4+ 45 Cu2+ 36 Ni2+ 30Co2+ 27 Al3+ 16 Ce3+ 5 Na+, Li+, K+, Mn2+, Ba2+, 0 Mg2+, Ba2+, Ca2+

A method of measuring a UK activity inhibiting rate is as follows:

A Tris-HCl buffer (pH7.5) was added to 20 μL of a suspension of a samplein water to a total about of 180 μL, 20 μL of 300 U/mL active type UK isadded thereto, and is allowed to stand at room temperature. After 30minutes, 20 μL of S2444 (CHROMOGENIX) which is a specific syntheticsubstrate for UK is added, and is further allowed to stand in a 37° C.thermostat for 30 minutes. Thereafter, 20 μL of a 12% aqueoustrichloroacetic acid solution is added to stop the reaction, a samplepowder is filtered, absorbance of the filtrate at 405 nm is measured toobtain UK activity in an assessment system, and a UK activity inhibitingrate of the sample is calculated.

Action of each ion on an enzyme has high specificity, and most excellentUK inhibiting activity is confirmed in zinc ion.

Further, when antibacterial and antifungal effect is considered, it ispreferable that the aforementioned zinc oxide and/or zinc basiccarbonate is a main component, and this contains 1 or more than 2 alkalimetal salts selected from hydroxide, hydrogencarbonate and, as carbonateof lithium, sodium and potassium as a mixture. In addition, it ispreferable that an alkali metal salt is particularly sodium carbonate orpotassium carbonate.

Inert Powder

As described above, the composite powder of the present invention mayhave a structure in which an adsorbing site and an acting site areformed on an inert powder (FIG. 2A). An inert powder is not particularlylimited as far as the effect of the present invention is notdeteriorated, and an inorganic base powder, an organic base powder, aninorganic pigment base powder, and a organic pigment base powder can beused.

Complex Effect

In a normal skin, PA is localized in the corneal layer and dermis.However, it is known that, by skin roughening and various skin diseasesaccompanied with keratinization abnormality, PA is activated, suitablelocalization of PA in the skin is disordered, and diffusion of PA isoccurred.

The reason why activation and diffusion of PA are inhibited by thecomposite powder of the present invention can be supposed as follows:

A substance with a negative zeta-potential value is excellent in abilityto electrically adsorb PA. When the composite powder having an adsorbingsite with a negative zeta-potential value is coated on skin, a largeamount of PA produced in the skin cell is attracted to the adsorbingsite, and is localized in an upper layer part of an epidermis. That is,PA is adsorbed on an adsorption site of the composite powder, anddiffusion is inhibited.

And, activation of PA adsorbed onto the adsorbing site of the compositepowder is inhibited by PA inhibiting effect of the acting site.

When trypsin that is classified into the same category of serineprotease as PA was studied as a reference, activity of trypsin washardly lost. That is, an acting site of the present invention does notinhibit enzyme activity non-specifically.

In PA, there are two kinds of urokinase (UK) and tissue type (PA). Theformer is a healthy epidermis, and the latter is recognized of itsexistence in a morbid epidermis mainly.

A representative of the composite powder of the present invention hasinhibitory activity on both of these PAs. It is preferable that PAinhibiting rate is 40% or more particularly 50% or more.

Even when powders constituting each site of the composite powder aremixed in the powder state, higher effect than that of each powder aloneis exerted depending on the condition in some cases. However, in acomposite powder in which a site having inhibitory activity on thesespecified enzymes, and an adsorbing site are exposed on a surface, sincemovement of a particle does not occur, an adsorbing site can continue tohave stably a negative zeta-potential, and extremely high enzymeactivity, for example, PA inhibiting effect is confirmed.

In addition, since the composite powder of the present invention useszinc oxide and/or zinc basic carbonate obtained by combing alkali metalsalts as an acting site, excellent antibacterial and antifungal effectis obtained as compared with zinc oxide which is a currently generallyused inorganic antibacterial agent. In addition, since zinc oxide and/orzinc basic carbonate and alkali metal salt are sufficiently mixed, andan alkali metal salt is encapsulated in a fine aggregate of zinc oxideand/or zinc basic carbonate, antibacterial and antifungal activity canbe continued for a long period, which is different from the case ofmixture of two agents in the powdery state.

The Process of Making the Composite Powder

An example of the process of making is shown in FIG. 4.

In this method, a composite powder can be effectively obtained by usinga base powder dispersion in addition to an aqueous solution containing azinc ion and an alkali aqueous solution, and reducing a time of waterwashing at a water washing step, in the aforementioned method ofsynthesizing zinc oxide and/or zinc basic carbonate, whereby, an alkalimetal salt adsorbed onto a fine particle of zinc oxide or zinc basiccarbonate dispersed in the reaction solution is intentionally made toremain.

First, an aqueous solution containing zinc ion, an alkali aqueoussolution, and a base powder dispersion are prepared. In FIG. 4, as abase powder dispersion (C), talc is used by dispersing in ion-exchangedwater. Further, as an aqueous solution containing a zinc ion (A), anaqueous zinc acetate solution is used and, as an alkali aqueous solution(B), an aqueous sodium carbonate solution is used.

An aqueous solution (A) containing zinc ion and an alkali aqueoussolution (B) are supplied to a reactor containing a base powderdispersion (C) under room temperature and atmospheric pressure whileamounts are adjusted so that pH of a reaction solution is retainedconstant 7 to 10, and the materials are mixed and stirred. Thus obtainedproduct can be centrifuged to filter it, washed with water, dried, andbaked. In an example of the process shown in FIG. 4, drying wasperformed at 105° C. for 12 hours in a drying step, and baking wasperformed at 300° C. in the baking step. In addition, in order to adjusta particle diameter of the powder, grinding treatment may be performedafter baking.

In synthesis of a composite powder, pH is preferably 7 to 10. When pH inthe synthesis is lower than 7 or exceeds 10, there is a possibility thatantibacterial and antifungal activity is not exerted.

As a raw material for an aqueous solution containing a zinc ion,inorganic acid salts such as zinc sulfate, zinc nitrate, zinc phosphate,zinc halide; organic acid salts such as zinc formate, zinc acetate, zincpropionate, zinc lactate, zinc oxalate, zinc citrate can be used.

In the present invention, it is particularly preferable to use zincacetate, zinc sulfate or zinc chloride. Further, when zinc sulfate orzinc chloride is used, it is preferable to add acetic acid whose molnumber is 2-fold of mol number of zinc contained in the material. Whenthese synthetic raw materials are used, antibacterial and antifungaleffect becomes particularly excellent.

As a raw material for an alkali aqueous solution, hydroxide,hydrogencarbonate, and carbonate of lithium, sodium, and potassium canbe used. In the present invention, it is particularly preferable to usesodium carbonate or potassium carbonate.

The process for preparing the composite powder of the present inventionis not limited to the aforementioned process, but any process can beapplied as far as the effect of the present invention is notdeteriorated.

For example, zinc oxide is directly synthesized without via zinc basiccarbonate using an aqueous solution of a strong alkali such as sodiumhydroxide and potassium hydroxide in place of an alkali aqueous solutioncontaining a carbonate ion, and this can be washed with water, filteredand dried to obtain a composite powder.

Alternatively, water washing is sufficiently performed in a waterwashing step of the aforementioned step, to synthesize a preliminarypowder (complex aggregate of zinc oxide and base powder) notsubstantially containing impurities other than a base powder and zincoxide, and the powder is immersed in an aqueous solution containing analkali metal salt, and dried, whereby, an alkali metal salt can beuniformly mixed in an alkali metal salt in a preliminary powder.

In the composite powder of the present invention, it is preferable thata content of zinc oxide and/or zinc basic carbonate is 5 to 75% byweight relative to a composite powder. When the content is less than 5%by weight, desired effect cannot be obtained in some cases and, when thecontent exceeds 75% by weight, spreading becomes difficult, and there isa possibility to deteriorate the usability when it is blended incosmetic compositions.

In addition, in the composite powder of the present invention, it ispreferable that a content of an alkali metal salt is 0.5 to 50% byweight of whole composite powder. When the content is less than 0.5% byweight, desired antibacterial and antifungal effect is not obtained insome cases, being not preferable. On the other hand, when the contentexceeds 50% by weight, although initial antibacterial activity is shownwell, the activity of a composition is deteriorated due to highhygroscopicity and dissolution out property of an alkali metal salt forelution out, or an antibacterial agent itself becomes strongly alkaline,being not preferable.

In addition, in the composite powder of the present invention, since analkali metal salt is present, excellent antibacterial and antifungaleffect is obtained as compared with zinc oxide, which is a currentlygenerally used inorganic antibacterial agent. In addition, since zincoxide and/or zinc basic carbonate and alkali metal salt are sufficientlymixed and an alkali metal salt is embedded in a fine aggregate of zincoxide and/or basic zinc oxide, antibacterial and antifungal activity canbe continued for long period unlike a mixture of the two powders in thesimple powdery state.

Further, by combining a base powder having better usability, spreadingbecomes easy when blended in cosmetic compositions.

In addition, it is preferable that pH of 10% by weight aqueousdispersion of the synthesized composite powder is 9 to 14, particularly9.5 to 12. When pH of an aqueous dispersion is less than 9, there is apossibility that antibacterial and antifungal activity in not exerted.

By inclusion of the aforementioned composite powder, the cosmeticcomposition of the present invention exhibits comprehensively excellentproperty over versatile elements such as antibacterial and antifungalproperty, safety and usability. And, since a preferable composite powderin the present invention does not use expensive raw material such assilver and zinc-substituted zeolite, the complex power is relativelyinexpensive as compared with the former inorganic antibacterial agent.In addition, unlike an agent utilizing photocatalystic function,antibacterial and antifungal effect can be also expected in dark place,and the composite powder has an advantage that an antibacterial agentalone or a composition containing an antibacterial agent has littlechange with time, which was frequently problematic in the formerantibacterial agent. Further, to mention specially, the composite powderexhibits high effect also on fungus such as mold and yeast against whichthe former inorganic antibacterial and antifungal agent has low effect.Thereby, the amount of an antiseptic such as paraben and sodiumdehydroacetate, which are generally used in cosmetic compositions to beblended, can be reduced, and cosmetic compositions without paraben,sodium dehydroacetate and so on have become possible. Although cosmeticcompositions such as mascara that are generally used around eyes requirestrong antiseptic effect, the amount of paraben is reduced, and theamount of an alcohol to be blended is suppressed by blending theaforementioned composite powder, whereby stimulation to the mucosa canbe reduced.

A content of the composite powder of the present invention contained inthe cosmetic of the invention is not particularly limited as far as theeffect of the invention can be obtained in the amount range, which canbe used by appropriately adjusting the amount. But the range isgenerally 0.5 to 60% by weight. When the content is less than 0.5% byweight, there is a possibility that the effect of the invention is notexerted. In some cases when the content exceeds 60% by weight, it is notpreferable from a viewpoint of preparation formulation.

Ingredients mentioned below which are used in normal cosmeticcompositions, for examples moisturizing agents, antioxidants, oilcomponents, ultraviolet absorbers, emulsifiers, surfactants, thickeners,alcohols, powder components, color materials, aqueous components, water,various kinds of skin nutrition agents and so on can be appropriatelyblended in the cosmetic of the present invention in such a range thatthe effect of the present invention is not deteriorated

Further, sequestering agents such as disodium edentate, trisodiumedentate, sodium citrate, poly sodium phosphate, metasodium phosphate,gluconic acid, malic acid and so on; various crude drug extracts such ascaffeine, tannin, verapamil, tranexamic acid and also the derivatives,licorice, Chinese quince, shinleaf and so on; agents such as tocopherolacetate, glycyrrhetinic acid, glycyrrhizinic acid and also thederivatives or the salts and so on; whitening agents such as vitamin C,magnesium ascorbate phosphate, ascorbic acid glucoside, arbutin, kojicacid and so on; amino acids such as arginine, lysine and also thederivatives; saccharides such as fructose, mannose, erythritol,trehalose, xylitol and so on can be also appropriately blended therein.

The cosmetic of the present invention can be applied in any form whichis used in the conventional cosmetic compositions, such as ointment,cream, milky lotion, lotion, pack, foundation, cheek rouge, eye shadow,face powder, lipstick, bath medicine, oil removing paper, paper facepowder, body powder, baby powder, powder spray and so on, a dosage formbeing not limited.

Application of the composite powder of this invention to sensitive skin,for which use of the former cosmetic compositions are difficult, showexcellent effect mentioned in the present invention.

A sensitive skin is defined in publications as follows:

“A skin usually susceptible to a damage due to a specific response toquasi-drugs, cosmetics, plants, ultraviolet ray, metals to which most ofhuman beings do not respond particularly.”

“A skin which is sensitive constitutionally to an allergenic substances(pollen, fragrance) or irritative substances (alcohols) due to a reducedbarrier function of skin.”

“A skin susceptible to a damage by an irritating substance onlytemporarily when the resistance of skin or the physiological functionsof skin are deteriorated due to an insufficient sleep, overwork,menstruation, seasons change, mental stress and the like.”

“A skin posing an anxiety about the use of cosmetics used routinely.”

Thus, factors for sensitive skin condition are reduced skin barrierfunction, reduced skin irritation threshold, skin dryness, substancecausing contact dermatitis, physicochemical irritation, stress, physicalcondition, seasons change, ultraviolet ray, menstruation and the like.It is also possible that one's mistaken skin care itself causes asensitive skin and that one's obsession just causes sensitive skin.

In the present invention, subject person having a sensitive skin isdefined as the person recognized abnormal felling in any of theprocedures (1) to (5) shown below.

(1) 100 μl of 5% aqueous solution of citric acid is applied over thecheek and allowed to stand for 10 minutes.

(2) 100 μl of 5% aqueous solution of lactic acid is applied over thecheek and allowed to stand for 10 minutes.

(3) 100 μl of 50% ethanol solution is applied over the cheek and allowedto stand for 10 minutes.

(4) An unwoven fabric (2×2 cm) is impregnated with 100 μl of 0.2%aqueous solution of methylparaben, and allowed to stand on the cheek for10 minutes.

(5) An unwoven fabric (2×2 cm) is impregnated with 100 μl of 5% aqueoussolution of SDS, and allowed to stand on the cheek for 10 minutes.

The abnormal felling means relatively painful feeling on skin, such astingling pain, creepy feeling, itching sensation, feverish feeling,discomfort, sting pain and the like.

Further, the composite powder of the present invention can be blendedinto all articles and member subjects which are directly contacted witha human skin, or may generate friction, such as paper articles andoffice supplies such as tissue paper, paper towel, napkin, bill, coupon,ticket, book, poster, newspaper, magazine, notebook, memo pad and so on;clothes such as lingerie, underwear, shirts, lining cloth of hats orshoes, socks, sandals and so on; childcare and nursing supplies such aspaper diaper for babies and infants and aged and so on; dailynecessaries such as sanitary products, contraceptive devices, kitchensponges, scrubbing brushes, toilet seat, toilet seat covers, dustcloths,toothbrushes, masks, medical use gauzes, band aids, medical usesupporter, softening agent, clothing use detergent and so on; furnitureand bedclothes such as chair, bed, bedding, blanket, Japanese cushion,pillow and their coverings, cabinet, curtain, carpet and so on;construction members such as wallpaper, wall material, floor material,pillar, handrail and so on; sport supplies such as handle and knob ofbaby car, cart, electric appliance, tableware, and shelf and so on; tapefor sports, supporter for sports and so on; grips and groves of varioussport supplies such as golf, tennis, table tennis and skiing, bats andgloves of baseball, and various protectors of rugby and football and soon; members such as vehicle sheets, strap, handle, interior articles ofautomobile, bicycle, bus, electric car and airplane and so on.

By blending the composite powder of the present invention, utilities asa functional raw materials which are very safe, highly reliable,effective on antibacterial and antifungal action, and effective on skinroughening suppressing or improving action are expected in daily lives,sport scenes or medical conducts.

EXAMPLE 1

Ion-exchanged water is placed into a reaction vessel, and 100 g of talc(JA-68R™: manufactured by ASADA SEIFUN CO., LTD., zeta-potential:−19.3mV) is dispersed therein. To this were connected two microtube pumps,and pH controller and a stirring apparatus were set. Two microtube pumpswere connected to each of a solution in which 33.4 g of zinc chlorideand 29.6 g of acetic acid were dissolved in 160 mL of ion-exchangedwater, and a solution in which 88.4 g of anhydrous sodium carbonate wasdissolved in 270 mL of ion-exchanged water, and fixed, so that eachsolution can be added dropwise to the reaction vessel. A reaction wasperformed by adjusting adding amounts of the two aqueous solutions,while stirring under atmospheric pressure and room temperature, and keptconstantly pH8 during the reaction. An addition dropwise time was about30 minutes. The resulting precipitates were washed with water, andfiltered three times repeatedly, dried in an oven at 105° C. for 12hours, ground with a personal mill, and baked at 300° C. for 1 hour.This powder was passed through a 60 mesh sieve after grinding, to obtainan objective material.

EXAMPLE 2

According to the same procedure as that of Example 1 except that mica(Eight pearl 300S™: manufactured by KAKUHACHI CO., LTD., zeta-potential:−18.9 mV) was used in place of talc in Example 1, an objective materialwas obtained.

EXAMPLE 3

According to the same procedure as that of Example 1 except that silica(CHEMISELEN™: manufactured by SUMITOMO CHEMICAL CO., LTD.,zeta-potential: −39.4 mV) was used in place of talc in Example 1, anobjective material was obtained.

EXAMPLE 4

Omitting the baking step in Example 1, a composite powder of zinc basiccarbonate was obtained.

EXAMPLE 5

According to the same procedure as that of Example 1 except that Alumina(MAX LIGHT A100™: manufactured by SHOWA DENKO K. K., zeta-potential:+17.3 mV) was used in place of talc in Example 1, an objective materialwas obtained.

EXAMPLE 6

According to the same procedure as that of Example 1 without blendingtalc, a composite of zinc oxide and sodium carbonate is obtained. 10 gof this composite and 50 g of talc were uniformly stirring to mix with asmall size mixer to obtain an objective mixture.

EXAMPLE 7

Zinc oxide on the market (manufactured by SEIDO CHEMICAL CO.,LTD)

EXAMPLE 8

Inorganic type antibacterial agent on the market (ZEOMIC™: manufacturedby SINANEN ZEOMIC CO.,LTD)

EXAMPLE 9

Talc (JA-68R™: manufactured by ASADA SEIFUN CO., LTD)

EXAMPLE 10

Mica (EIGHT PEARL 300S™: manufactured by KADOHACHIGYORINHAKU CO., LTD)

EXAMPLE 11

Silica(CHEMISELEN™: SUMITOMO CHEMICAL K.K.)

1. Antibacterial and Antifungal Activity Test

FIG. 5 is a view for explaining a method of assessing antibacterial andantifungal activity. For the test of fungi, a potato dextrose agarmedium was used, and for the test of bacteria, room bouillon agar mediumwas used. As shown in FIG. 5, a medium 24 is made in a laboratory dish22, and each test bacterial strain of fungi[Blue mold (Penicillium sp.),Black mold (Aspergillus niger), Candida albicans (Candida albicansATCC10231)]; and bacteria [Pseudomonas aeruginosa (Pseudomonasaeruginosa ATCC15442), Escherichia coli (Escherichia coli ATCC8739),Staphylococcus aureus (Staphylococcus aureus FDA209P), Acne germ(P.acnes JCM6473)] is coated on the medium 24. A sample 26 obtained bycompressing and molding each powder of Example 1 to 11 into a disc of 8mm diameter with a pharmacy compressing machine is disposed on a centerof the medium 24, a fungus is cultured at 25° C. for 72 hours, abacterium is cultured at 30° C. for 48 hours, and activity thereof wasassessed by a width 28 of a growth inhibiting band, in which growth ofeach fungus or bacterium was inhibited, formed around a sample 26 on themedium 24 after a predetermined time. It can be estimated that as awidth 28 of a growth inhibiting band is wider, antibacterial andantifungal activity is excellent. And, activity was assessed byevaluation criteria as shown in Table 1.

2. Measurement of PA Inhibitory Activity

A Tris-HCl buffer (pH 7.5) was added to each 20 μL of a suspension of apowder of Example 1 to 11 to a total amount of 180 μL, and 20 μL of 300U/mL active-type urokinase (UK) was added thereto, and allowed to standat room temperature. After 30 minutes, 20 μL of S2444 (CHROMOGENIX)which is a synthetic substrate specific for UK was added, and this wasfurther allowed to stand in a thermostat at 37° C. for 30 minutes.Thereafter, 20 μL of a 12% aqueous trichloroacetic acid solution wasadded to stop the reaction, a sample powder was filtered, absorbance ofthe filtrate at 405 nm was measured to obtain PA activity in theestimating system, and the PA inhibiting rate of a sample wascalculated. When the PA inhibiting rate is 40% or higher, it isestimated that there is PA inhibiting activity. UK is one kind of PA asdescribed above.

The result is shown in Table 2.

TABLE 1 Evaluation criteria Evalu- Width of the growth Width of thegrowth ation prevention band of fungi prevention band of bacteria A 15.0mm or more 7.5 mm or more B 10.0 mm or more less than 5.0 mm or moreless than 15.0 mm 7.5 mm C 5.0 mm or more less than 2.5 mm or more lessthan 10.0 mm 5.0 mm D Less than 5.0 mm Less than 2.5 mm E 0 mm (withoutinhibiting 0 mm (without inhibiting band) band)

TABLE 2 PA inhibiting Antibacterial and antifungal activity Example rate(%) (1) (2) (3) (4) (5) (6) (7) 1 51 A A A B B A A 2 55 A A A C B A A 353 A A A C B A A 4 47 A A B C B A A 5 28 A A A C C A A 6 26 A A A C C AA 7 34 E D D E D D C 8 18 D D D B B B B 9 15 E E E E E E E 10 16 E E E EE E E 11 20 E E E E E E E (1) Blue mold (2) Black mold (3) Candidaalbicans (4) Pseudomonas aeruginosa (5) Escherichia coli (6)Staphylococcus aureus (7) Acne germRegarding Antibacterial and Antifungal Activity

Example 7 with only zinc oxide was inferior in both of antibacterial andantifungal activity as compared with Examples 1 to 4, which are usingthe composite powder of the present invention. From this, it was seenthat although zinc oxide was originally known as an inorganicantibacterial substance, sufficient antibacterial and antifungalactivity cannot be obtained only with itself and, by combining an alkalimetal salt with zinc oxide, antibacterial and antifungal activity isimproved. In addition, also in Example 8, which is a commerciallyavailable inorganic antibacterial agent, antibacterial and antifungalactivity was inferior as compared with Examples 1 to 4 which are usingthe composite powder of the present invention.

In addition, also in the composite of zinc basic carbonate without afiring step (Example 4), the same effect as that of the composite ofzinc oxide (Examples 1 to 3) was recognized.

Further, in Example 5 using alumina having a positive zeta-potential,antibacterial and antifungal activity against Escherichia coli was loweras compared with Examples 1 to 4 using talc, mica or silica having anegative zeta-potential. In addition, also in Example 6 in which acomposite of zinc oxide and alkali metal salt, and talc were merelymixed, antibacterial and antifungal activity against Escherichia coliwas low.

Regarding PA Inhibitory Activity

In Example 5 using alumina having a positive zeta-potential as anadsorbing site, a PA inhibiting rate was lower as compared with Examples1 to 4 using talc, mica or silica having a negative zeta-potential as anadsorbing site. This can be thought that because of positivezeta-potential, PA cannot be adsorbed.

In addition, also in Example 7 with only zinc oxide, a PA inhibitingrate was inferior. From this, it was seen that although zinc oxide wasoriginally known to have skin roughening improving effect, sufficient PAinhibiting activity cannot be obtained only with itself and, bycombining with an adsorbing site having PA adsorbing activity, PAinhibiting effect is improved.

In addition, in Examples 9 to 11 using talc, mica, or silica alone, a PAinhibiting rate was inferior. Therefore, it was confirmed that PAinhibitory activity can not be obtained by adsorbing site only.

In addition, in Example 6 in which merely mixing an acting with talcacted as an adsorbing site causes a low PA inhibiting rate, and it wasconfirmed that, by combining an adsorbing site with an acting site asshown in Examples 1 to 4, remarkable improvement of the inhibiting ratewas seen. This is thought that merely mixing an adsorbing site with anacting site causes movement of a particle, so that an adsorbing site cannot have a negative potential stably.

Therefore, it was confirmed that antibacterial and antifungal effect ofthe composite powder of the present invention is improved by combiningzinc oxide with a salt of an alkali metal. In addition, the compositepowder has effect also on acne bacterium, and has effect of inhibitingpimple. Further, it was confirmed that, by combining an adsorbing sitehaving a negative zeta-potential with an acting site, excellent PAinhibitory activity is exerted.

Then, a specific method of testing antibacterial and antifungalactivity, stimulating property, and easy spreading of a cosmeticcomposition containing the composite powder of the present invention, aswell as Evaluation criteria will be explained below.

Antibacterial and Antifungal Activity

Test method: Each sample is molded in an inner dish based on JIS Z2911mold resistance test, a mold is sprayed, the dish is covered with a lid,and allowed to stand in a constant temperature incubator at 25° C. undermoisturing condition, and the presence or the absence of growth of amold is observed with naked eyes.

Evaluation Criteria

-   ∘: After 4 weeks, a hypha is not seen with naked eyes.-   Δ: After 4 weeks, a hypha is slightly observed with naked eyes-   ×: After 4 weeks, a hypha is widely observed with naked eyes    Stimulating Property

Test method: A sample was coated on 20 panelists, and they werequestioned whether they feel stimulation after 10 minutes.

Evaluation Criteria

-   ∘: No panelists felt stimulation.-   Δ: 1 panelist felt stimulation.-   ×: 2 or more panelists felt stimulation.    Easiness of Spreading

Test method: function evaluation was performed by 20 specialist aspanelists.

Evaluation Criteria

-   ⊚(easy): 8 or more panelists felt easy.-   ∘(slightly easy): 5 to 7 panelists felt easy.-   Δ(slightly difficult): 2 to 4 panelists felt easy.-   ×(difficult): 1 or less panelist felt easy.

A process for preparing a cosmetic composition is as follows:

An oily phase part is mixed at 85° C., sprayed to an uniformly mixedpowder part, and the materials are mixed with a blender.

Results are shown in Table 3.

TABLE 3 Blending example Sample(wt %) 1 2 3 4 5 6 7 8 9 10 Example 1 5 —— — — — — — — — Example 2 — 5 — — — — — — — — Example 3 — — 5 — — — — —— — Example 6 — — — — — — — — — 5 Example 7 — — — 5 — — — — — — Example8 — — — — 5 — — — — — Ethyl paraben — — — — — 0.5 — — — — Talc 20 20 2020 20 20 25 — 20 20 Mica 63 63 63 63 63 67.5 63 5 63 63 Silica — — — — —— — — 5 — Dimethylpoly- 1 1 1 1 1 1 1 1 1 1 siloxane Diisostearyl 5 5 55 5 5 5 5 5 5 malate Glyceryl 5 5 5 5 5 5 5 5 5 5 trioctanoate Sorbitan1 1 1 1 1 1 1 1 1 1 sesquioleate Antibacterial and ◯ ◯ ◯ X X ◯ X X X ◯anitfungal activity Stimulating ◯ ◯ ◯ ◯ ◯ X ◯ ◯ ◯ ◯ property Easiness of◯ ◯ ◯ X X ◯ ◯ ◯ ◯ X spreading

As apparent from Table 3, Blending Example 4 using commerciallyavailable zinc oxide, and Blending Example 5 using a commerciallyavailable antibacterial and antifungal agent had no stimulation, butwere inferior in antibacterial and antifungal activity, and easyspreading property. Blending Example 6 using ethylparaben hadantibacterial and antifungal activity and easy spreading, but wasinferior in stimulation. Blending Examples 1 to 3 using the compositepowder of the present invention exhibited sufficient antibacterial andantifungal activity without blending ethylparaben, and had easyspreading property, and no stimulation.

In addition, it was seen that cosmetic composition in Blending Examples1 to 3 using the composite powder of the present invention also exhibitantibacterial and antifungal activity to acne bacterium, and are alsoeffective on a pimpled skin.

In addition, powders obtained in Examples 1 to 4 were analyzed byfluorescent X-ray, X-ray diffraction and infrared absorptionspectroscopy indicated that the acting site is composed of zinc oxide asa main ingredient, together with 2 to 15% by weight of sodium carbonate.

Study of Synthetic Raw Material for Zinc Oxide and/or Zinc BasicCarbonate

Subsequently, the influence of difference in raw zinc compound for zincoxide and/or zinc basic carbonate which is contained in the acting sitestudied on PA inhibitory activity and antibacterial and antifungalactivity.

EXAMPLE 12

Ion-exchanged water is placed into a reaction vessel, and 100 g of talc(JA-68R™: manufactured by ASADA SEIFUN CO., LTD., zeta-potential:−19.3mV) is dispersed thererin. To this were connected two microtube pumps,and pH controller and a stirring apparatus were set. Two microtube pumpswere connected to each of a solution in which 50.1 g of zinc chlorideand 44.4 g of acetic acid were dissolved in 240 mL of ion-exchangedwater, and a solution in which 130 g of anhydrous sodium carbonate wasdissolved in 400 mL of ion-exchanged water, and fixed, so that eachsolution can be added dropwise to the reaction vessel. A reaction wasperformed by adjusting amounts of two aqueous solutions to be addeddropwise, while stirring under atmospheric pressure and roomtemperature, and kept constantly pH10 during the reaction. An additiondropwise time was about 30 minutes. The resulting precipitates werewashed with water, and filtered three times repeatedly, dried in an ovenat 120° C. for 12 hours, ground with a personal mill, and fired at 450°C. for 1 hour. This powder was passed through a 60 mesh sieve aftergrinding, to obtain an objective material.

EXAMPLE 13

According to the same procedure as that of Example 12 except that “59.3g of zinc sulfate” was used in place of “50.1 g of zinc chloride” inExample 12, an objective material was obtained.

EXAMPLE 14

According to the same procedure as that of Example 12 except that “81.0g of zinc acetate” was used in place of “50.1 g of zinc chloride and44.4 g of acetic acid” in Example 12, an objective material wasobtained.

EXAMPLE 15

According to the same procedure as that of Example 12 except that aceticacid was removed.

EXAMPLE 16

According to the same procedure as that of Example 12 except that “24.5g of sodium hydroxide” was used in place of “130 g of anhydrous sodiumcarbonate” in Example 12, and that acetic acid was removed, an objectivematerial was obtained.

EXAMPLE 17

According to the same procedure as that of Example 12 except that “90 gof anhydrous sodium carbonate” was used in place of “130 g of anhydroussodium carbonate” in Example 12, and that acetic acid was removed, anobjective material was obtained.

PA inhibitory activity and antibacterial and antifungal activity ofpowders obtained in Examples 12 to 16 were tested by the above methodand criteria.

The result is shown in Table 4.

TABLE 4 PA inhibiting Antibacterial and antifungal activity Example rate(%) (1) (2) (3) (4) (5) (6) 12 52 A A A A A A 13 51 A A A B A A 14 53 CB A D D D 15 52 E D D E D D 16 51 E D D E D D (1) Blue mold (2) Blackmold (3) Candida albicans (4) Pseudomonas aeruginosa (5) Escherichiacoli (6) Staphylococcus aureus

It was apparently seen from Table 4 that in each example, PA inhibitingrate was excellent. In addition the powders of Examples 12 to 14 haveexcellent antibacterial and antifungal activity to each test microbialas compared with those of Examples 15 and 16. Therefore, it ispreferable to use zinc acetate, zinc sulfate or zinc chloride as a rawmaterial for synthesizing zinc oxide and/or zinc basic carbonate. And itis preferable that when zinc sulfate or zinc chloride is used as a rawmaterial, it is preferable to add acetic acid to zinc (mole number;acetic acid/zinc=2).

Further, antibacterial and antifungal activity was tested for cosmeticcompositions containing powders obtained in Examples 12, 13, 14, 16 and17.

The result is shown in Table 5.

TABLE 5 Blending example Sample(wt %) 11 12 13 14 15 Example 12 5 — — —— Example 13 — 5 — — — Example 14 — — 5 — — Example 17 — — — 5 — Example16 — — — — 5 Mica 20 20 20 20 20 Silica 63 63 63 63 63Dimethylpolysiloxane 1 1 1 1 1 Diisostearyl malate 5 5 5 5 5 Glyceryltrioctanoate 5 5 5 5 5 Sorbitan sesquioleate 1 1 1 1 1 Stimulatingproperty ◯ ◯ ◯ ◯ ◯ Easiness of spreading ◯ ◯ ◯ ◯ ◯ Antibacterial and ◯ ◯◯ X X antifungal activity

It was apparently seen from Table 5 that cosmetic compositions ofBlending examples 11 to 13 have excellent antibacterial and antifungalproperty as compared with cosmetic compositions of Blending examples 14and 15. Therefore, it was confirmed also in powder-blended cosmeticcompositions that it is preferable to use zinc acetate, zinc sulfate orzinc chloride as a raw material for synthesizing zinc oxide. And whenzinc sulfate or zinc chloride is used, it is preferable to add aceticacid to zinc at double mole number.

Zinc acetate is relatively expensive as an industrial material, but itwas seen that even when a material different from zinc acetate is usedas a raw material for synthesizing zinc oxide, by adding acetic acid ata mole number which is 2-fold a mole number of zinc, a powder havingmore excellent antibacterial and antifungal activity over that of apowder synthesized using zinc acetate as a synthesis material can besynthesized.

When acetic acid is not used, an alkali metal salt is flown out bywashing of a powder, effect is reduced to half.

Content of Zinc Oxide and/or Zinc Basic Carbonate

Subsequently, the influence by content of zinc oxide was studied for PAinhibitory activity, antibacterial and antifungal property and usefeeling.

EXAMPLE 18

Ion-exchanged water is placed into a reaction vessel, and 100 g of talc(JA-24R™: manufactured by ASADA SEIFUN CO., LTD., zeta-potential:−17.0mV) is dispersed therein. To this were connected two microtube pumps,and pH controller and a stirring apparatus were set. Two microtube pumpswere connected to each of a solution in which zinc chloride and aceticacid were dissolved in ion-exchanged water, and a solution in whichanhydrous sodium carbonate was dissolved in ion-exchanged water, andfixed so that each solution can be added dropwise to the reactionvessel. Each solution changed as Table 6. A reaction was performed byadjusting amounts of two aqueous solutions to be added dropwise, whilestirring under atmospheric pressure and room temperature, and keptconstantly pH10 during the reaction. An addition dropwise time was about30 minutes. The resulting precipitates were washed with water, andfiltered three times repeatedly, dried in an oven at 105° C. for 12hours, ground with a personal mill, and fired at 300° C. for 1 hour.This powder was passed through a 100 mesh sieve after grinding, toobtain an objective material having different contents of zinc oxide.These are designated as Examples 18-2 to 18-11 depending on a content ofzinc oxide, as described in Table 6.

EXAMPLE 18-1

Talk (JA-24R™: manufactured by ASADA SEIFUN CO., LTD)

TABLE 6 Zinc solution Alkali solution Content of Ion Zinc Acetic IonAnhydrous zinc oxide exchanged chloride acid exchanged sodium carbonate(wt %) water (mL) (g) (g) water (mL) (g) Example 18-2 1 8 1.67 1.48 13.54.42 Example 18-3 5 40 8.35 7.4 67.5 22.1 Example 18-4 10 80 16.7 14.8135 44.2 Example 18-5 20 160 33.4 29.6 270 88.4 Example 18-6 30 240 50.144.4 405 132.6 Example 18-7 40 320 66.8 59.2 540 176.8 Example 18-8 50400 83.5 74 675 221 Example 18-9 60 480 100.2 88.8 810 265.2 Example18-10 75 600 125.25 111 1012.5 331.5 Example 18-11 90 720 150.3 133.21215 397.8

PA inhibitory activity, antibacterial and antifungal activity andeasiness of spreading of powders obtained in Examples 18-1 to 18-11 weretested by the above method and criteria.

The result is shown in Table 7.

TABLE 7 Content of PA inhibiting Antibacterial and antifungal activityEasiness of Example zinc oxide (%) rate (%) (1) (2) (3) (4) (5) (6)spreading 18-1 0 20 E E E E E E ◯ 18-2 1 30 E E D E E E ◯ 18-3 5 42 D DB D E D ◯ 18-4 10 47 C C A D D B ◯ 18-5 20 53 A A A A B A ◯ 18-6 30 55 AA A A A A ◯ 18-7 40 54 A A A A A A ◯ 18-8 50 55 A A A A A A ◯ 18-9 60 54A A A A A A ◯ 18-10 75 53 A A A A A A ◯ 18-11 90 54 A A A A A A X (1)Blue mold (2) Black mold (3) Candida albicans (4) Pseudomonas aeruginosa(5) Escherichia coli (6) Staphylococcus aureus

As seen from Table 7, at a content of zinc oxide of 5% by weight orlarger, a PA inhibiting rate was increased, and antibacterial andantifungal activity was also improved. However, in Example 18-11containing zinc oxide at 90% by weight, spreading was difficult, andthere is a possibility that usability at blending in a cosmeticcomposition is deteriorated. From the forgoing results, a content ofzinc oxide is preferably 5 to 75% by relative to the whole compositepowder.

Further, antibacterial and antifungal activity, stimulating property andeasiness of spreading of cosmetic compositions containing powdersobtained in Examples 18-2 to 18-11 were tested. Result is shown in Table8.

TABLE 8 Blending example 16- Sample(wt %) 1 2 3 4 5 6 7 8 9 10 Example18-2 5 — — — — — — — — Example 18-3 — 5 — — — — — — — — Example 18-4 — —5 — — — — — — — Example 18-5 — — — 5 — — — — — — Example 18-6 — — — — 5— — — — — Example 18-7 — — — — — 5 — — — — Example 18-8 — — — — — — 5 —— — Example 18-9 — — — — — — — 5 — — Example 18-10 — — — — — — — — 5 —Example 18-11 — — — — — — — — — 5 Talc 20 20 20 20 20 20 20 20 20 20Mica 63 63 63 63 63 63 63 63 63 63 Dimethylpolysiloxane 1 1 1 1 1 1 1 11 1 Diisostearyl malate 5 5 5 5 5 5 5 5 5 5 Glyceryl trioctanoate 5 5 55 5 5 5 5 5 5 Sorbitan sesquioleate 1 1 1 1 1 1 1 1 1 1 Antibacterialand Δ ◯ ◯ ◯ ◯ ◯ ◯ ◯ ◯ ◯ antifungal activity Stimulating property ◯ ◯ ◯ ◯◯ ◯ ◯ ◯ ◯ ◯ Easiness of spreading ◯ ◯ ◯ ◯ ◯ ◯ ◯ Δ Δ X

As seen from Table 8, cosmetic compositions containing composite powdersin Examples 18-2 to 11 having a content of 5% by weight of zinc oxide orlarger showed high antibacterial and antifungal activity. However, in acosmetic composition containing the composite powder in Example 18-11containing 90% by weight of zinc oxide, spreading was difficult. Fromthe forgoing results, it was also confirmed in powder-blended cosmeticcomposition that a content of zinc oxide is preferably 5 to 75% byweight relative to the whole composite powder.

Content of Alkali Metal Salt

Subsequently, what differences are produced in PA inhibitory activityand antibacterial and antifungal activity by an amount of an alkalimetal salt was studied.

EXAMPLE 19

Ion-exchanged water is placed into a reaction vessel, and 100 g of talc(JA-68R™: manufactured by ASADA SEIFUN CO., LTD., zeta-potential:−19.3mV) is dispersed therein. To this were connected two microtube pumps,and pH controller and a stirring apparatus were set. Two microtube pumpswere connected to each of a solution in which 33.4 g of zinc chlorideand 29.6 g of acetic acid were dissolved in 160 mL of ion-exchangedwater, and a solution in which 36 g of sodium hydroxide was dissolved in400 mL of ion-exchanged water, and fixed, so that each solution can beadded dropwise to the reaction vessel. A reaction was performed byadjusting amounts of two aqueous solutions to be added dropwise, whilestirring under atmospheric pressure and room temperature, and keptconstantly pH 8 during the reaction. An addition dropwise time was about30 minutes. The resulting precipitates were washed with water, andfiltered three times repeatedly, dried in an oven at 105° C. for 12hours, ground with a personal mill, and fired at 300° C. for 1 hour.This powder was passed through a 60 mesh sieve after grinding, to obtainan objective preliminary powder (composite powder of talc and zincoxide).

The aforementioned preliminary powder was added to an aqueous solutionin which sodium carbonate was dissolved in 20 mL of ion-exchanged water,the materials were sufficiently stirred and mixed with a homomixer, anddried using an oven at 110° C. for 14 hours to obtain an objectivematerial. A mixing amount of sodium carbonate and a preliminary powderwas changed as shown in Table 9, to obtain composite powders havingdifferent contents of an alkali metal salt.

TABLE 9 Mixed quantity (g) Sodium carbonate Preliminary Sodium contentpowder carbon (wt %) Example 19-1 10 0 0 Example 19-2 9.975 0.025 0.25Example 19-3 9.95 0.05 0.50 Example 19-4 9.9 0.1 1.00 Example 19-5 9.750.25 2.50 Example 19-6 9.5 0.5 5.00 Example 19-7 9 1 10.00 Example 19-87.5 2.5 25.00 Example 19-9 5 5 50.00 Example 19-10 2.5 7.5 75.00 Example19-11 0 10 100.00

PA inhibitory activity and antibacterial and antifungal activity ofpowders obtained in Examples 19-1 to 19-11 were tested by the abovemethod and criteria. The result is shown in Table 10.

TABLE 10 Content of PA inhibiting sodium carbonate rate Antibacterialand antifungal activity Example (%) (%) (1) (2) (3) (4) (5) (6) 19-1 052 E E D E D D 19-2 0.25 53 E D D E D D 19-3 0.5 52 D D B D C D 19-4 151 C C B D C C 19-5 2.5 53 A A A C B B 19-6 5 52 A A A A B A 19-7 10 53A A A A A A 19-8 25 51 A A A A A A 19-9 50 35 A A A A B A 19-10 75 15 AA A A B A 19-11 100 10 D B A A B A (1) Blue mold (2) Black mold (3)Candida albicans (4) Pseudomonas aeruginosa (5) Escherichia coli (6)Staphylococcus aureus

As apparent from Table 10, at a content of sodium carbonate of 50% byweight or larger, as a content of sodium carbonate was increased, a PAinhibiting rate was decreased.

Little antibacterial and antifungal activity was seen in Example 19-1composed of only a preliminary powder and, at a content of sodiumcarbonate of 0.5% by weight or larger, as the content was increased, theactivity was improved. However, at a content of sodium carbonate of 75%by weight or larger, deterioration in activity of a composition due tohigh hygroscopicity and dissolution out property of sodium carbonate,and influence of an antibacterial agent itself on a human body due tostrong alkali property are feared. Further, in Example 19-11 containing100% by weight of sodium carbonate, the effect on blue mold and blackmold was decreased.

From this result, it was confirmed that a content of an alkali metalsalt is preferably 0.5 to 50% by weight of the whole composite powder.

Based on this result, when a preliminary powder and an alkali metal saltwere simply mixed in the powder state, it was found out antibacterialand antifungal activity is improved. However, although betterantibacterial property is exhibited at an early stage, it was confirmedthat an alkali metal salt easily dissolved out, and the effect does notcontinue. For this reason, in order that antibacterial and antifungalactivity continues over a long term, it is preferable that zinc oxideand an alkali metal salt are sufficiently mixed, and an alkali metalsalt is encapsulated in a fine aggregate of zinc oxide.

Further, antibacterial and antifungal activity, stimulating property andeasiness of spreading of cosmetic compositions containing powdersobtained in Examples 19-1 to 19-11 were tested. The result is shown inTable 11.

TABLE 11 Blending example 17- Sample(wt %) 1 2 3 4 5 6 7 8 9 10 11Example 19-1 5 — — — — — — — — — — Example 19-2 — 5 — — — — — — — — —Example 19-3 — — 5 — — — — — — — — Example 19-4 — — — 5 — — — — — — —Example 19-5 — — — — 5 — — — — — — Example 19-6 — — — — — 5 — — — — —Example 19-7 — — — — — — 5 — — — — Example 19-8 — — — — — — — 5 — — —Example 19-9 — — — — — — — — 5 — — Example 19-10 — — — — — — — — — 5 —Example 19-11 — — — — — — — — — — 5 Talc 20 20 20 20 20 20 20 20 20 2020 Mica 63 63 63 63 63 63 63 63 63 63 63 Dimethylpoly- 1 1 1 1 1 1 1 1 11 1 siloxane Diisostearyl 5 5 5 5 5 5 5 5 5 5 5 malate Glyceryl 5 5 5 55 5 5 5 5 5 5 trioctanoate Sorbitan 1 1 1 1 1 1 1 1 1 1 1 sesquioleateAntibacterial and X Δ Δ ◯ ◯ ◯ ◯ ◯ ◯ ◯ Δ antifungal activity Stimulating◯ ◯ ◯ ◯ ◯ ◯ ◯ ◯ ◯ Δ X property Easiness of ◯ ◯ ◯ ◯ ◯ ◯ ◯ ◯ ◯ Δ Δspreading

As apparent from Table 11, little antibacterial and antifungal activitywas seen in Example 19-1 containing only a preliminary powder and, at acontent of sodium carbonate 0.5% by weight or larger, the effect wasexerted. However, in Example 19-10 containing 100% by weight of sodiumcarbonate, the effect was decreased. In particular, at a content ofsodium carbonate of 1 to 75% by weight, the effect was better. Inaddition, at a content of sodium carbonate of 75% by weight or larger, apossibility that activity of a composition is deteriorated due to highhygroscopicity and dissolution out of sodium carbonate, or anantibacterial agent itself becomes strong alkaline property is feared.

From this result, it was confirmed that a content of an alkali metalsalt is preferably 0.5 to 50% by weight of the whole composite powderalso in a powder-blended cosmetic composition.

pH at Synthesis and pH of Aqueous Dispersion

FIG. 6 shows a relationship between antifungal activity on blue mold,and pH of an aqueous dispersion when a composite powder was dispersed inwater into a 10% by weight slurry. Antifungal activity is expressed by awidth of a growth inhibition band by the aforementioned method. As shownin the same figure, it is seen that a powder having high moldproofingproperty has pH of an aqueous dispersion of 9 to 14, particularly 9.5 to12. Therefore, pH of a 10% by weight aqueous dispersion is preferably 9to 14, most preferably 9.5 to 12.

In addition, it was found that pH at synthesis is greatly involved in afactor of increasing pH of a dispersion of a powder in water. That is,it was seen that when pH upon synthesis of a composite powder iscontrolled at 7 to 10, a dispersion of a synthesized powder in watertends to exhibit pH of 9 to 14.

Then, a relationship between pH at synthesis, and PA inhibitory activityand antibacterial and antifungal activity was studied in detail.

EXAMPLE 20

Ion-exchanged water is placed into a reaction vessel, and 100 g of talc(FIT POWDER FK-300S™: manufactured by YAMAGUCHI MICA CO.,zeta-potential:−19.3 mV) is dispersed thererin. To this were connectedtwo microtube pumps, and a pH controller and a stirring apparatus wereset. Two microtube pumps were connected to each of a solution in which66.8 g of zinc chloride and 59.2 g of acetic acid were dissolved in 320mL of ion-exchanged water, and a 33% of anhydrous sodium carbonateaqueous solution, and fixed so that each solution can be added dropwiseto the reaction vessel. A reaction was performed by adjusting amounts oftwo aqueous solutions to be added dropwise, while stirring underatmospheric pressure and room temperature, and kept constantly pH asTable 12 during the reaction. The resulting precipitates were washedwith water, and filtered three times repeatedly, dried in an oven at105° C. for 12 hours, ground with a personal mill, and fired at 300° C.for 1 hour. This powder was passed through a 100 mesh sieve aftergrinding, to obtain an objective material.

These are designated as Examples 20-1 to 20-5 depending on pH atsynthesis, as described in Table 12.

EXAMPLE 20-6

Talk (FIT POWDER FK-300S™)

TABLE 12 Alkali solution pH at Ion-exchange Sodium carbonate synthesiswater (mL) anhydrous (g) Example 20-1 6 350 115.5 Example 20-2 7 440145.2 Example 20-3 8 540 176.8 Example 20-4 9 720 235.2 Example 20-5 101020 386.8

PA inhibitory activity and antibacterial and antifungal activity ofpowders obtained in Examples 20-1 to 20-6 were tested by the abovemethod and criteria, and the relation with the pH at synthesis wereinvestigated.

The result is shown in Table 13.

TABLE 13 pH at PA syn- inhibiting Antibacterial and antifungal activityExample thesis rate (%) (1) (2) (3) (4) (5) (6) 20-1 6 35 A A A A A A20-2 7 43 A A A A A A 20-3 8 52 A A A A A A 20-4 9 53 A A A D D B 20-510 54 C C D D D E 20-6 11 53 D D D E E E 20-7 — 25 E E E E E E (1) Bluemold (2) Black mold (3) Candida albicans (4) Pseudomonas aeruginosa (5)Escherichia coli (6) Staphylococcus aureus

From Table 13, PA inhibiting rate was increased when pH at synthesis was7 to 11, and antibacterial and antifungal activity was excellent when pHat synthesis was 6 to 10. From the forgoing results, pH at synthesis ispreferably 7 to 10. This is thought because pH of dispersion ofsynthesized powder in water tends to exhibit to be 9 to 14 when pH atsynthesis is controlled at 7 to 10, PA inhibitory activity andantibacterial and antifungal activity become excellent as describedabove.

And, it was seen that, in the present invention, all powders exhibitingbetter PA inhibitory activity and antibacterial and antifungal activityexhibit pH of 9 to 14 when prepared into 10% by weight aqueousdispersion. Therefore, in the present invention, pH of 10% by weight ofcomposite powder in aqueous dispersion is preferably 9 to 14.

Studies were further performed in detail for antibacterial andantifungal activity, stimulating property and spreading property ofcosmetic compositions of the present invention.

The result is shown in Table 14.

TABLE 14 Blending example Sample(wt %) 18 19 20 21 22 Sodium carbonate-5 4 — — — containing-zinc oxide covering talc Sodium carbonate- — — — —5 containing-zinc oxide Ethylparaben — 0.1 0.1 0.5 — Talc 21 21.9 25.925.5 21 Mica 62 62 62 62 62 Dimethylpolysiloxane 1 1 1 1 1 Diisostearylmalate 5 5 5 5 5 Glyceryl trioctanoate 5 5 5 5 5 Sorbitan sesquioleate 11 1 1 1 Antibacterial and ◯ ◯ X ◯ ◯ antifungal activity Stimulatingproperty ◯ Δ Δ X ◯ Easiness of spreading ◯ ◯ ◯ ◯ Δ

As apparent from Table 14, Blending example 20 containing 0.1% by weightof ethylparaben showed easy spreading property but no antibacterial andantifungal activity. In order to obtain antibacterial and antifungalactivity, it was necessary to blend ethylparaben at 0.5% by weight asseen in Blending example 21. However, in the case of Blending example 18containing 5% by weight of the composite powder of the presentinvention, sufficient antibacterial and antifungal activity wasexhibited without ethylparaben. Further, spreading was easy, andusability was better. In addition, in Blending example 19 containing 4%by weight of the composite powder of the present invention, even when anamount of ethylparaben is reduced to 0.1% by weight, better easyspreading and antibacterial and antifungal activity are possessed. Inaddition, in Blending example 22 using sodium carbonate-containing zincoxide, which is not combined with a base powder, inferior easiness ofspreading was observed.

Since the composite powder of the present invention does not use anexpensive raw material such as silver- and zinc-substituted zeolite, itis inexpensive as compared with the conventional inorganic antibacterialagent. The composite powder of the present invention has advantage inproblems which were frequently observed in the conventionalantibacterial agent. That is, time-dependent changes such asdiscoloration and color degradation of antibacterial agent itself orcomposition containing the antibacterial agent are little. Further, tostate specially, the composite powder of the present invention exhibitshigh effect also on fungi such as mold and yeast against which theconventional inorganic antibacterial and antifungal agent had loweffect.

Embodiment 1 Cream (prescription) wt % 1) Stearic acid monoglyceride 2.02) Stearyl alcohol 4.0 3) Bee wax 3.0 4) Lanolin 5.0 5) P.O.E (20 mol)sorbitan monooleate 2.0 6) Squalane 20.0 7) Sodiumcarbonate-containing-zinc 5.0 oxide covering talc 8) perfume 0.2 9)1,3-Butylene glycol 5.0 10)  Glycerol 5.0 11)  Purified water remainder(process)

1) to 6) and 8) are heated and kept at 75° C. (oily phase). 9) and 10)are dissolved in 11), added and dispersed 7) and heated to 75° C.(aqueous phase). The aqueous phase is added to the oily phase andemulsified homogeneously with a homomixer, and cooled down to 30° C.with sufficient stirring.

Embodiment 2 Baby powder (prescription) wt % 1) Talc 80.4 2) Calciumcarbonate 17.0 3) Starch 0.5 4) Sodium carbonate-containing-zinc 2.0oxide silica complex 5) Antiseptics 0.1 (process)

1) to 5) are stirred to mix well with a blender.

Embodiment 3 Emulsifying foundation (prescription) wt % 1) Stearic acid0.4 2) Isostearic acid 0.3 3) Cetyl 2-ethylhexanoate 4.0 4) Liquidparaffin 11.0 5) P.O.E (10) stearyl ether 2.0 6) Talc 15.0 7) Red ironoxide 0.01 8) Yellow iron oxide 0.001 9) Black iron oxide 0.05 10) Cetyl alcohol 0.3 11)  Lithium hydroxide-containing-zinc 5.0 oxidecovering silica 12)  Triethanolamine 0.4 13)  Dipropylene glycol 5.014)  Perfume 0.01 15)  Purified water remainder (process)

After 1) to 10) are heated to 85° C. to dissolve them, 11) is added anduniformly dispersed. Into this, a mixture of 12), 13) and 15) which hadbeen heated to 85° C. to dissolve them, gradually added to emulsify. Theemulsion is stirred keeping the emulsification temperature for 10minutes, and cooled to 45° C. while stirring. To this, 14) is added, themixture is continuously cooled to 35° C. while stirring, and this ischarged into a container.

Embodiment 4 Pack (prescription) wt % 1) Polyvinyl alcohol 15.0 2)Polyethylene glycol 3.0 3) Propylene glycol 7.0 4) Ethanol 10.0 5)Sodium carbonate-containing-zinc 10.0 oxide covering silica 6) Perfume0.1 7) Purified water remainder (process)

2) and 3) are added to 7) to dissolve them. Next 1) is added, heated anddissolved, and 5) is dispersed. Added 4) and 6) to dissolved them whilestirring.

Embodiment 5 Solid powder foundation (prescription) wt % 1) Sericite22.0 2) Synthesis mica 15.0 3) Talc remainder 4) Sodiumcarbonate-containing-zinc 7.0 oxide covering silica 5) Ferric oxide 0.86) Yellow iron oxide 2.0 7) Black iron oxide 0.1 8) Zinc white 2.0 9)Silicone elastic powder 2.0 10)  Spherical polyethylene 4.0 11) Dimethylpolysiloxane 3.0 12)  Liquid paraffin 5.0 13)  Vaseline 5.0 14) Sorbitan sesquiisostearate 1.0 15)  Anti-oxidant proper quantity 16) Perfume proper quantity (process)

1) to 16) are stirred to mix well with a blender.

Embodiment 6 W/O type emulsified makeup foundation (prescription) wt% 1) Cyclomethicone 30.0 2) Dimethicone 2.0 3) Silicone resin 1.0 4)Antioxidant proper quantity 5) Octyl methoxy cinnamate 3.0 6) 4-tertbutyl-4′-methoxy 1.0 benzoylmethane 7) Isostearic acid 1.0 8) Siliconetreated alumina 8.0 9) Cation modified bentonite 2.0 10)  Sodiumcarbonate-containing-zinc 5.0 oxide covering talc 11)  Talc 5.0 12) Spherical PMMA resin powder 5.0 13)  Purified water remainder 14) Glycerol 4.0 15)  1,3-Propylene glycol 1.0 16)  Stabilizer properquantity 17)  Perfume proper quantity (process)

1) to 9), 12), 16) and 17) are heated to 85° C. to dissolve them, and10) and 11) are added and dispersed (oily phase). 14) and 15) are addedto 13), and are uniformly dispersed (aqueous phase). An oily phase isadded to an aqueous phase, this is stirred while retaining at 85° C. for100 minutes, and cooled to 45° C. while stirring.

Embodiment 7 W/O style emulsifying foundation (prescription) wt %  1)Silicone treated synthesis mica 15.0  2) Silicone treated sericite 7.0 3) Silicone treated titanium oxide 12.0  4) Silicone treated ferricoxide 1.2  5) Silicone treated yellow iron oxide 2.3  6) Siliconetreated black iron oxide 0.6  7) Potassiumhydrogencarbonate-containing-zinc 12.0 oxide covering mica  8) SphericalPMMA powder 4.0  9) Cyclomethicone remainder 10) Dimethylpolysiloxane4.0 11) Squalane 3.0 12) Polyether modifed silicone 2.0 13) Sorbitansesqui isostearate 1.0 14) Dispersant Proper quantity 15) Dipropyleneglycol 2.0 16) Phenoxyethanol 0.1 17) Purified water 20.0 18)Antioxidant proper quantity 19) Perfume proper quantity (process)

1) to 14) are heated to 85° C. to dissolve them (oily phase). 16) isadded to 17), and are uniformly dispersed (aqueous phase). An oily phaseis added to an aqueous phase, this is stirred while retaining at 85° C.for 100 minutes, added 18) and 19), and cooled to 45° C. while stirring.

Embodiment 8 White powder (prescription) wt % 1) Talc remainder 2)Synthesis mica 22.0 3) Sodium hydroxide-containing-zinc 13.0 oxidecovering talc 4) Spherical silicone powder 4.0 5) Squalane 3.0 6)Perfume proper quantity (process)

1) to 5) are stirred to mix well with a blender, and 6) is sprayeduniformly.

Embodiment 9 O/W type emulsifying foundation (prescription) wt % 1)Sericite 17.0 2) Mica 20.0 3) Lithium carbonate-containing-zinc 8.0oxide covering mica 4) Ferric oxide 0.3 5) Yellow iron oxide 1.2 6)Black iron oxide 0.6 7) Spherical polyethylene powder 6.0 8) Squalane10.0 9) Olive oil 10.0 10)  Stearic acid 2.0 11)  Glyceryl monostearate2.0 12)  Sorbitan POE (40) monostearate 2.0 13)  Glycerol 5.0 14) Hexane 1,2-diol 1.0 15)  Triethanolamine 0.8 16)  pH modifier properquantity 17)  Purified water remainder (process)

1) to 12) are heated to 85° C. to dissolve them (oily phase). 13) to 16)are added to 17), and are uniformly dispersed (aqueous phase). An oilyphase is added to an aqueous phase, this is stirred while retaining at85° C. for 100 minutes and cooled to 45° C. while stirring.

Embodiment 10 O/W type emulsifying makeup foundation (prescription) wt% 1) Purified water remainder 2) Glycerol 20.0 3) Pentane 1,2-diol 3.04) 1,3-Butylene glycol 1.0 5) Liquid paraffin 7.5 6) Isostearic acid 0.57) Ascorbic acid (whitening agent) 0.2 8) Matricaria extract (whiteningagent) 0.1 9) Saxifrage extract (whitening agent) 0.3 10)  di2-Ethylhexyl phthalate 0.3 11)  Spherical silica 4.0 12)  Sodiumcarbonate-containing-zinc 5.0 oxide covering talc 13)  Talc 5.0 14) Stabilization agent proper quantity 15)  Perfume proper quantity(process)

5) to 14) are heated to 85° C. to dissolve them (oily phase). 2) to 4)are added to 1), and are uniformly dispersed and heated to 85° C.(aqueous phase). An oily phase is added to an aqueous phase, this isstirred while retaining at 85° C., added 15) and cooled to 45° C. whilestirring.

Embodiment 11 Two-way powder foundation (prescription) wt % 1) Siliconetreated sericite 13.0 2) Silicone treated mica remainder 3) Siliconetreated talc 15.0 4) Potassium carbonate-containing-zinc 5.0 oxidecovering mica 5) Aluminum stearate treated fine 6.0 particle titaniumoxide 6) Silicone treated titanium oxide 9.0 7) Silicone treated ferricoxide 1.2 8) Silicone treated yellow iron oxide 2.5 9) Silicone treatedblack iron oxide 0.9 10)  Barium sulfate powder 7.0 11)  Polyurethanepowder 1.0 12)  Silicone elastic powder 5.0 13)  Polyethylene powder 2.014)  Interference titanated mica 4.0 15)  Dimethylpolysiloxane 3.0 16) Methyl phenyl polysiloxane 2.0 17)  Vaseline 2.0 18)  Octyl methoxycinnamate 3.0 19)  Sorbitan sesuqui isostearate 1.0 20)  Polyethersilicone 1.0 21)  Antioxidant proper quantity 22)  Perfume properquantity (process)

1) to 21) are heated 85° C. while stirring, and then 22) is sprayeduniformly.

Embodiment 12 Two-way powder foundation (prescription) wt % 1) Fluorinemodified silicone treated sericite 22.0 2) Fluorine modified siliconetreated mica remainder 3) Fluorine modified silicone treated kaolin 10.04) Potassium hydrogencarbonate containing zinc 7.0 oxide covering silica5) Silicone treated fine particle titanium oxide 8.0 6) Fluorinemodified silicone treated titanium oxide 9.0 7) Fluorine modifiedsilicone treated ferric oxide 1.2 8) Fluorine modified silicone treatedyellow iron oxide 2.5 9) Fluorine modified silicone treated black ironoxide 0.9 10)  Spherical silicone powder 8.0 11)  Lauroyl lysinecovering titanium oxide 4.0 12)  Dimethylpolysiloxane 4.0 13) Polyethylene glycol 2.0 14)  Fluoro polyether 2.0 15)  Octylmethoxycinnamate 2.0 16)  Sorbitan sesuqui isostearate 1.0 17) Antioxidant proper quantity 18)  Perfume proper (process) quantity

1) to 17) are heated 85° C. while stirring, and then 18) is sprayeduniformly.

Embodiment 13 Wipe substance for cleaning (prescription) wt % 1)Purified water 91.945 2) Salt (Japanese pharmacopoeia) 0.35 3)Dipropylene glycol 2.0 4) Sodium hexa metaphosphate 0.005 5) Sodiumhydrogencarbonate-containing-zinc 5.0 oxide covering talc 6) Bentonite0.5 7) POE (20) octyl dodecyl ether 0.1 (process)

2) to 7) are dissolved and dispersed in 1) while well stirring, andsoaked into nonwoven fabric.

Embodiment 14 Paper powder (prescription) wt % 1) Colorant 25 2) Sodiumcarbonate-containing-zinc 3 oxide covering silica 3)Carboxymethylcellulose sodium 0.2 4) Sodium metaphosphate 0.2 5)Polyoxyethylene sorbitan monooleate 0.2 (20E. O.) 6) Perfume 0.1 7)Common water proper quantity Total 100 wt % (process)

The coating solution that mixed 1) to 6) in 7) are coated on the paper,and dried.

The cosmetic compositions of Embodiments 1 to 14 have excellentantibacterial and antifungal activity and have no stimulating property.

Embodiment 15 Adhesion to Leather, Timber or the Like

The composite powder of the present invention was printed with a bindermade of a synthetic resin, and followed by heat treatment to adhere thecomposite powder by the resin. By these procedures, antibacterial andantifungal effect, and skin roughening inhibiting and improving effectare exerted.

Embodiment 16 Coating on Glass, Metal or the Like

By adding the composite powder of the present invention to an adhesive,and coating this, antibacterial and antifungal effect, and skinroughening inhibiting and improving effect are exerted.

An outline of the process is as follows:

-   -   1. A slurry of the composite powder of the present invention is        prepared.    -   2. An adhesive (oxidized starch, resin, resin emulsion etc.) is        added.    -   3. This is uniformly coated, and dried.

Embodiment 17 Filling into Paper, Fiber or the Like

A paper is an extremely rough porous sheet, which is originally madefrom a main raw material of a plant fiber. When the composite powder ofthe present invention is filled therein, the powder is retained in theinterior. Then antibacterial and antifungal effect, and skin rougheninginhibiting and improving effect are exerted.

An outline of the process is as follows.

-   -   1. A pulp is dispersed in water, and fibers are cut with a        beater to convert into viscous.    -   2. The composite powder of the present invention is added as        filler.    -   3. This is subjected to a paper making machine.

Embodiment 18 Blending into Garment Detergent or Softness FinishingAgent, or the Like

By blending the composite powder of the present invention into a garmentdetergent or a softness finishing agent, the composite powder is adheredto a garment to be contacted with a skin, and retained therein. Thenantibacterial and antifungal effect, and skin roughening inhibiting andimproving effect are exerted.

Embodiment 19 Blending into Powder Product

In powder products such as body powder and powder spray, it wasdifficult to be blended liquid component such as water and oil. Byblending the composite powder of the present invention into such powderproduct, antibacterial and antifungal effect and skin rougheninginhibiting and improving effect, which could not be expected previously,are exerted.

Embodiment 20 Blending into Paste, Varnish, Lacquer, Paint or the Like

By mixing the composite powder of the present invention into a materialsuch as paste, varnish, lacquer and paint, antibacterial and antifungaleffect, and skin roughening inhibiting and improving effect are exertednot only in materials itself, but also in materials coated or adhered bysaid powder.

As explained above, according to the composite powder and the cosmeticcomposition of the present invention, excellent antibacterial andantifungal property can be obtained by inclusion of zinc oxide and/orzinc basic carbonate, and alkali metal salt.

Further, a composite powder having plasminogen activator inhibitoryactivity in addition to antibacterial and antifungal effect can beobtained by combining an acting site comprising zinc oxide and/or zincbasic carbonate and an alkali metal salt with an adsorbing site.

1. A composite powder having antibacterial and antifungal effectcomprising: a base powder; wherein said base powder provides anadsorbing site for adsorbing a specified enzyme; a zinc oxide and/orzinc basic carbonate; and an alkali metal salt; wherein said zinc oxideand/or zinc basic carbonate and said alkali metal salt are combined asan acting site to inhibit an activity of said enzyme which is adsorbedby said adsorbing site of said base powder; wherein said base powder,said zinc oxide and/or zinc basic carbonate, and said alkali metal saltare combined; and wherein said alkali metal salt is encapsulated in saidzinc oxide and/or the zinc basic carbonate, wherein said base powder isat least one selected from the group consisting of silica, talc, mica,polyamide, polymethyl methacrylate and silicone resin; and wherein saidalkali metal salt is at least one selected from the group consisting oflithium hydroxide, sodium hydroxide, potassium hydroxide, lithiumhydrogen carbonate, sodium hydrogen carbonate, potassium hydrogencarbonate, lithium carbonate, sodium carbonate and potassium carbonate.2. The composite powder according to claim 1, wherein a surface of saidbase powder is covered with said zinc oxide and/or zinc basic carbonateand said alkali metal salt.
 3. The composite powder according to claim2, wherein said surface of said base powder is covered with said zincoxide and/or zinc basic carbonate and said alkali metal salt in a stripeor spot state or in a net state.
 4. The composite powder according toclaim 1, wherein said zinc oxide and/or zinc basic carbonate and saidalkali metal salt are encapsulated, embedded or included in said basepowder.
 5. The composite powder according to claim 1, wherein the actingsite and the adsorbing site are formed on an inactive powder in a stripeor spot state.
 6. The composite powder according to claim 1, whereinsaid specified enzyme is a plasminogen activator, and said acting sitehas an inhibitory effect on said plasminogen activator.
 7. The compositepowder according to claim 1, wherein said adsorbing site of said basepowder has a zeta potential at a negative value at a skin pH when saidspecified enzyme is a plasminogen activator.
 8. The composite powderaccording to claim 1, wherein said adsorbing site of said base powderhas a zeta potential at −10 mV or lower at pH 7.5 when said specifiedenzyme is a plasminogen activator.
 9. The composite powder according toclaim 1, wherein said alkali metal salt is at 0.5 to 50% by weight ofthe composite powder.
 10. The composite powder according to claim 1,wherein said zinc oxide and/or zinc basic carbonate is at 5 to 75% byweight of the composite powder.
 11. The composite powder according toclaim 1, wherein said zinc oxide and/or zinc basic carbonate issynthesized by zinc acetate, zinc chloride or zinc sulfate with thepresence of acetic acid.
 12. The composite powder according to claim 6,wherein said acting site has an inhibitory rate of 40% or more onplasminogen activator when said plasminogen activator is absorbed bysaid absorbing site on said base powder of the composite powder.
 13. Thecomposite powder according to claim 1, wherein a 10% by weight of thecomposite powder has a pH 9 to 14 when dispersed in water to exertantibacterial and antifungal activity.
 14. A cosmetic compositioncomprising the composite powder according to claim
 1. 15. The cosmeticcomposition according to claim 14, wherein said cosmetic compositiondoes not contain other antibacterial and antifungal agent.
 16. Thecomposite powder according to claim 1, wherein said base powder issilica and said alkali metal salt is sodium carbonate.
 17. A method forpreparing the composite powder of claim 1, comprising: supplying anaqueous solution containing said zinc oxide and/or zinc basic carbonateand an aqueous alkali solution containing said alkali metal salt to areactor containing a base powder to form a reaction solution; adjustingsaid reaction solution with said aqueous solution containing said zincoxide and/or zinc basic carbonate and said zinc ion and said aqueousalkali solution containing said alkali metal salt to adjust a pH tobetween 7 to 10 under room temperature and an atmospheric pressure toform a pH adjusted composite powder solution; filtering said pH adjustedcomposite powder solution to form a filtered composite powder; andwashing said filtered composite powder with water followed by drying toform said composite powder.